Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation

Goodman, A. J.; Tisdale, W. A.

doi:10.1103/physrevlett.114.183902

Title: Enhancement of Second-Order Nonlinear-Optical Signals by Optical Stimulation

Journal Article · Wed May 06 00:00:00 EDT 2015 · Physical Review Letters

DOI:https://doi.org/10.1103/physrevlett.114.183902· OSTI ID:1505727

Goodman, A. J. ^[1]; Tisdale, W. A. ^[2]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemical Engineering

Second-order nonlinear optical interactions such as sum- and difference-frequency generation are widely used for bioimaging and as selective probes of interfacial environments. However, inefficient nonlinear optical conversion often leads to poor signal-to-noise ratio and long signal acquisition times. We demonstrate the dramatic enhancement of weak second-order nonlinear optical signals via stimulated sum- and difference-frequency generation. We present a conceptual framework to quantitatively describe the interaction and show that the process is highly sensitive to the relative optical phase of the stimulating field. To emphasize the utility of the technique, we demonstrate stimulated enhancement of second harmonic generation (SHG) from bovine collagen-I fibrils. Using a stimulating pulse fluence of only $$3\text{ }\text{ }\mathrm{nJ}/{\mathrm{cm}}^{2}$$, we obtain an SHG enhancement >$${10}^{4}$$ relative to the spontaneous signal. The stimulation enhancement is greatest in situations where spontaneous signals are the weakest—such as low laser power, small sample volume, and weak nonlinear susceptibility—emphasizing the potential for this technique to improve signal-to-noise ratios in biological imaging and interfacial spectroscopy.

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Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0010538; 1122374

OSTI ID:: 1505727

Alternate ID(s):: OSTI ID: 1179710

Journal Information:: Physical Review Letters, Vol. 114, Issue 18; ISSN 0031-9007

Publisher:: American Physical Society (APS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 15 works

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